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Then my top 5 are:
1. Higurashi no Naku Koro Ni (Kai/Rei)
2. Code Geass
3. Vampire Knight
4. Shakugan No Shana
5. Record of Lodoss War (newer series, the OVA sucked)
Oh, and I just realised 4/5 of these are japanese+subbed

In no particular order:

Big O!
Martian Successor Nadesico
Tengen Toppa Gurren Lagann
Giant Robo
Shin Mazinger Shōgeki! Z-Hen
King of Braves Gaogaigar
Heat Guy J

And probably others that I've forgotten.